Bulk Carrier Recombination Mechanisms and Photovoltage Deficit in Kesterite Solar Cells

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Hai Ma, Qiang Zhu, Long Zou, Bin Xu, Hongru Wang, Rui Ge, Fangyu Yue, Yuanyuan Zhang, Lin Sun, Ye Chen, Junhao Chu
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Abstract

Significant open-circuit voltage deficit (VOC-def) is regarded as the primary obstacle to achieving efficient kesterite solar cells. By leveraging a synergistic approach that combines photoluminescence, admittance spectroscopy and cathodoluminescence techniques, the theoretical models of radiative recombination in Cu2ZnSnS4 kesterite are revisited, allowing for a comprehensive clarification of both radiative and nonradiative recombination loss effects of VOC-def in the kesterite bulk and at interfaces. This quantitative analysis of VOC-def reveals that Cu/Zn disorder remains a fundamental limitation for kesterite solar cells, comparable to deep-level defects. Specifically, it is demonstrated that the asymmetric photoluminescence band commonly observed in Cu2ZnSnS4 consists of two competing components: tail-impurity recombination (conduction band → CuZn) and quasi-donor-acceptor-pair recombination (ZnCu → CuZn). These findings confirm that Cu/Zn antisite defects and related potential fluctuations reduce the effective bandgap. Furthermore, it is confirmed that band tails in kesterite are the result of electrostatic potential fluctuations and bandgap fluctuations. The amplitude of the electrostatic potential fluctuations is estimated to be ≈30 meV. Bandgap fluctuations in kesterite are experimentally distinguished from electrostatic potential fluctuations for the first time, which leads to a bandgap contraction of about 130 meV. These studies provide crucial theoretical support for the advancement of kesterite photovoltaic technology.

Abstract Image

Kesterite太阳能电池的散体载体重组机制和光电压缺陷
严重的开路电压亏缺(VOC-def)被认为是实现高效kesterite太阳能电池的主要障碍。通过结合光致发光、导纳光谱和阴极发光技术的协同方法,重新审视了Cu2ZnSnS4 kesterite中辐射复合的理论模型,从而全面澄清了kesterite体和界面处VOC-def的辐射和非辐射复合损失效应。这种voco -def的定量分析表明,Cu/Zn无序仍然是kesterite太阳能电池的基本限制,与深层缺陷相当。具体来说,在Cu2ZnSnS4中常见的不对称光致发光带由两个相互竞争的组分组成:尾部杂质复合(导带→CuZn)和准供体-受体-对复合(ZnCu→CuZn)。这些发现证实了Cu/Zn对位缺陷和相关的电位波动降低了有效带隙。进一步证实了kesterite中的带尾是静电电位波动和带隙波动的结果。静电电位波动的幅度估计为≈30 meV。首次通过实验将kesterite中的带隙波动与静电电位波动区分开来,从而导致约130 meV的带隙收缩。这些研究为kesterite光伏技术的发展提供了重要的理论支持。
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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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